Spin density distribution of the conduction electrons in diperylene hexafluorophosphate analysed by high-resolution NMR

High-resolution ¹³C nuclear magnetic resonance with ¹H cross polarization and ¹H decoupling under magic angle spinning is measured for the quasi-one dimensional organic conductor diperylene hexafluorophosphate (including tetrahydrofurane solvent molecules) at temperatures between 160 K and 270 K. Ab initio molecular orbital calculations are used for chemical shift analysis and for assignment of Knight shifted lines and individual carbon positions. The coexistence of neutral perylene molecules and perylene radicals in the same radical cation salt is revealed. From Knight and chemical shifts we were able to distinguish two inequivalent perylene radicals within the conducting stack. The spin density distribution of the molecular electronic wave function is determined quantitatively for these radicals. Received 29 June 1999 and Received in final form 4 November 1999